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Substrate‐Induced Synthesis of Nitrogen‐Doped Holey Graphene Nanocapsules for Advanced Metal‐Free Bifunctional Electrocatalysts
Authors:Zheye Zhang  Tengfei Cao  Shasha Liu  Xianming Duan  Li‐Min Liu  Shuai Wang  Yunqi Liu
Institution:1. Key laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, China;2. Beijing Computational Science Research Center, Beijing, China;3. State Key Laboratory of Digital Manufacturing Equipment and Technology, Huazhong University of Science and Technology, Wuhan, China;4. Beijing National Laboratory for Molecular Sciences Institute of Chemistry, Chinese Academy of Sciences, Beijing, China
Abstract:The development of efficient metal‐free electrocatalysts for oxygen electrocatalysis is of great significance for various energy conversion devices. Herein, novel nitrogen‐doped holey graphene nanocapsules (NHGNs) are reported prepared by self‐assembly of graphene oxide nanosheets on the surface of amino‐functionalized silica template and NH3 activation with simultaneously enhanced nitrogen doping and etching of nanopores in graphene, followed by template etching. The silica template is demonstrated to show a substrate‐enhanced effect on nitrogen doping and etching of nanopores in graphene based on density functional theory calculations. Benefiting from the large surface area, unique pore distribution, and high surface functionality of nitrogen doping, the resulting NHGNs exhibit superior bifunctional electrocatalytic activity and durability for both oxygen reduction reaction and oxygen evolution reaction, which is similar to that of the commercial Pt/C and RuO2 electrocatalysts, respectively. This work presents an advance in developing new nitrogen‐doped graphene species for highly efficient metal‐free electrocatalysis.
Keywords:bifunctional electrocatalysts  density functional theory calculations  nitrogen‐doped holey graphene nanocapsules  oxygen electrocatalysis  substrate enhanced effects
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